Reaction mechanisms of sodium carbonate activation in ultra-high-volume slag-cement blends

Abstract

Ultra-high-volume slag-cement (UHVS) blends can substantially reduce clinker ratio, but slow slag reaction limits strength development; Na2CO3 is a less caustic and lower-carbon activator for alkali-activated materials, yet its moderate alkalinity can similarly delay strength development. Here, dry-blended Na2CO3 (0-20 wt.% relative to water) was incorporated into a one-part binder with 90 wt.% ground-granulated blast-furnace slag and 10 wt.% Portland cement (PC) to determine whether this integration could mitigate slow strength development in both systems. Compressive strength testing, isothermal calorimetry, time-resolved quantitative X-ray diffraction, Fourier-transform infrared spectroscopy, aqueous solution analysis, and thermodynamic modeling were combined to determine how Na2CO3 controls phase assemblage, alkalinity, calculated porosity and strength development. At 5-10 wt.% Na2CO3, calcite-dominated carbonate reactions promoted a rapid alkalinity increase and accelerated early-age reaction and strength development; however, subsequent alkalinity decline limited later-age slag reaction and gel formation. In contrast, 20 wt.% Na2CO3 favored substantial early formation of gaylussite and carbonate-AFm phases, which moderated the initial pH rise and delayed early gel accumulation. The larger alkali inventory and evolving phase-solution partitioning helped sustain alkalinity at later ages, enabling continued slag dissolution and gel formation. This pathway produced higher reaction extent and lower calculated porosities, with compressive strength approaching that of neat PC. Screening-level cradle-to-gate life-cycle assessment indicates a 66-72% reduction in global warming potential relative to PC, depending on Na2CO3 production pathways. These results identify carbonate-mediated control of alkalinity persistence as key to sustaining slag reaction in UHVS systems.